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Portable water splitting devices driven by rechargeable metal–air batteries or solar cells are promising, however, their scalable usages are still hindered by lack of suitable multifunctional electrocatalysts. Here, a highly efficient multifunctional electrocatalyst is demonstrated, i.e., 2D nanosheet array of Mo‐doped NiCo2O4/Co5.47N heterostructure deposited on nickel foam (Mo‐NiCo2O4/Co5.47N/NF)...